Due to the high radiotoxicity in high concentrations, plutonium isotopes have drawn high attentions in the consideration of radiation risk, their sources, level, environmental behaviors, including deposition, retention and migration behaviors. However, such research in the Qinghai-Tibet Plateau is still missing, where is deemed as an environmental sensitive area. ²³⁹,²⁴⁰Pu in surface soil collected from the Qinghai-Tibet Plateau were determined for the first time in this work. The concentrations of ²³⁹,²⁴⁰Pu are in the range of 0.0176–1.95 Bq/kg, falling into the reported ranges in the background areas from the similar latitude belt. The ²⁴⁰Pu/²³⁹Pu atomic ratio range was measured to be 0.146–0.225, which is similar with the global fallout values. Both indicate that the global fallout is the major source of plutonium in this region, and the low plutonium level will not cause any radiation risk so far. Based on the statistical analysis of the possible parameters (organic content, moisture content, average annual precipitation, altitudes, topography and human activity), the large variations of ²³⁹,²⁴⁰Pu concentrations were mainly attributed to the retention process related factors including soil organic content and human activity disturbances. While, the deposition related factors including the average annual precipitation, altitudes, topography made insignificant influence on the spatial distribution of ²³⁹,²⁴⁰Pu concentrations due to the low ²³⁹,²⁴⁰Pu concentrations in atmosphere, less wet deposition amount and insignificant re-suspended amount. The highest ²³⁹,²⁴⁰Pu concentrations of 0.805–1.95 Bq/kg were mainly due to the good retention condition in the sampling sites with higher soil organic content and less human activity disturbances.

Concentrations of ²³⁹Pu and ²⁴⁰Pu in 163 surface soil samples and five soil cores collected from the northeast and north China were analyzed using the radiochemical separation combined with inductively coupled plasma mass spectrometry measurement. The average ²⁴⁰Pu/²³⁹Pu atomic ratios (0.185 ± 0.018) for all surface soil samples indicated that the global fallout is the major source of plutonium in the studied region. The ²³⁹,²⁴⁰Pu concentrations of the surface soil ranged from 0.002 mBq/g to 4.82 mBq/g, lying in the range of the reported results in the areas with similar latitude, except for a few samples. The distribution of ²³⁹,²⁴⁰Pu in this region is controlled by the deposition of plutonium in the atmosphere and its preservation in the soil, which were affects by multi-factors such as topography, climate, utilization of the land and vegetation coverage. The analytical results could be used as the baseline data for the assessment of the impact of nuclear activities in the past and the future.

Plutonium in the environment has drawn significant attentions due to its radiotoxicity in high concentration and source term linked with nuclear accidents and contaminations. The isotopic ratio of plutonium is source dependent and can be used as a fingerprint to discriminate the sources of radioactive contaminant. ²³⁹Pu, ²⁴⁰Pu and ¹³⁷Cs in surface soil and soil cores collected from Northern Xinjiang were determined in this work. The concentrations of ²³⁹,²⁴⁰Pu and ¹³⁷Cs are in the range of 0.06–1.20 Bq kg⁻¹, and <1.0–31.4 Bq kg⁻¹ (decay corrected to Sep. 2017), respectively, falling in the ranges of global fallout in this latitude zone. The ²⁴⁰Pu/²³⁹Pu atomic ratios of 0.118–0.209 and ²³⁹,²⁴⁰Pu/¹³⁷Cs activity ratios of 0.039–0.215 were measured. Among the investigated sites, distinctly lower ²⁴⁰Pu/²³⁹Pu atomic ratios of 0.118–0.133 and higher ²³⁹,²⁴⁰Pu/¹³⁷Cs activity ratios of 0.065–0.215 compared to the global fallout values were observed in the northwest part, indicating a significant contribution from other source besides the global fallout. This extra source is mainly attributed to the releases of atmospheric nuclear weapons testing at Semipalatinsk Nuclear Test Site, which was transported by the west and northwest wind through the river valley among mountains in this region. This contribution is estimated to account for 28–43% of the global fallout in the northwest part of Northern Xinjiang. The contribution from the Chinese atmospheric nuclear weapons testing to this region is negligible due to the lack of appropriate wind direction to transport the radioactive releases to this region.

Studies on the distribution and isotope compositions of fallout Pu are important for source characterization of possible future non-fallout Pu contamination in aquatic environments, and useful for dating of recent sediments to understand the pollution history of environmental contaminants. We present the historical record of atmospheric Pu fallout reconstructed from a sediment core from Lake Hongfeng, China. The Pu activity profile was in agreement with the 137Cs profile. Inventories were 50.7 Bq m-2 for 239+240Pu and 1586 Bq m-2 for 137Cs. The average 240Pu/239Pu atom ratio was 0.185 ± 0.009, indicating that Pu originated from global stratospheric fallout rather than from direct tropospheric or close-in fallout from the Chinese nuclear testing conducted in the 1970s. Our data suggested that Lake Hongfeng would be an ideal setting for monitoring atmospheric fallout and environmental changes in this region. Fallout Pu recorded in sediments can be used for quick dating of recent sediments to understand the pollution history of environmental contaminants.

The spatial distribution of plutonium isotopes (²³⁹Pu, ²⁴⁰Pu) in the surface sediments collected from the northwestern South China Sea (SCS) in 2018 was investigated. The ²³⁹,²⁴⁰Pu concentrations in surface sediments vary from 0.048 to 0.960 mBq/g (with mean of 0.282 ± 0.242 mBq/g) depending on the geographical feature of the sampling location such as the river estuary, continental shelf, slope and deep basin. Higher ²⁴⁰Pu/²³⁹Pu atomic ratios (0.24–0.31) in the surface sediment of the SCS compared to the global fallout value of 0.18 were observed, this is attributed to the input of close-in fallout of the Pacific Proving Ground (PPG) transported by the North Equatorial Current and Kuroshio Current to the northern SCS. The contribution of the PPG derived plutonium in the SCS sediment was estimated to be 39%–78% using a simple two-end member mixing model based on the measured ²⁴⁰Pu/²³⁹Pu atomic ratios in the sediment. Besides the soluble ²³⁹,²⁴⁰Pu level in seawater, load of suspended particulate matter from the river runoff and biological debris, hydrographic and hydrodynamic conditions are key parameters influencing the deposition process of plutonium to the sediment.

The spatial distributions of mercury (Hg) and zinc (Zn) concentration and the isotopic composition of plutonium (Pu) were investigated in surface sediments and sediment cores collected from the Southern Yellow Sea (SYS) during May 2014. The variation of the ²⁴⁰Pu/²³⁹Pu atom ratio (0.18–0.31) in the surface sediments of the SYS clearly indicated a signal of close-in fallout input from the Pacific Proving Ground (PPG). The buried ²³⁹⁺²⁴⁰Pu in the sediment of the SYS was estimated to be (4.7 ± 0.5) × 10¹⁰ Bq y⁻¹ during the period from 2011 to 2014, of which ∼33% (1.5 × 10¹⁰ Bq y⁻¹) was derived from the PPG by long-range transport via ocean currents (e.g., the North Equatorial Current and Kuroshio Current). The concentrations of Hg and Zn varied from 0.003 to 0.067 mg kg⁻¹ and from 43.9 to 137 mg kg⁻¹, respectively, and exhibited positive correlations with the ²³⁹⁺²⁴⁰Pu activity both in the surface sediments (0–1 cm) and upper layers (7 cm) of the sediment cores. Therefore, by using Pu as a tracer, we estimated that the oceanic input contributed 2.0 tons y⁻¹ of Hg and 1.0 × 10³ tons y⁻¹ of Zn to the SYS sediments between 2011 and 2014, which accounted for 33% and 3% of total buried Hg and Zn, respectively. These findings indicate that environmental pollution control should also consider the oceanic contribution of some pollutants. The results of the present work help to elucidate the biogeochemical cycling of trace metals in marginal seas, and are helpful for managing environmental pollution in marine environments.

In order to investigate the sources of plutonium in seawaters of Liaodong Bay and Bohai Strait, China, surface seawater samples were collected and analyzed for 239+240Pu and 137Cs by radiochemical separation combined with ICP-MS and γ-spectrometry, respectively. A large variation of 239+240Pu activities was observed, ranging from 1.993 to 29.677 mBq/m3 in the Liaodong Bay and from 0.932 to 10.183 mBq/m3 in the Bohai Strait. 137Cs activities showed little variation between the investigated locations, which was attributed to the different behavior characteristics of 239+240Pu and 137Cs in seawaters. The 240Pu/239Pu atom ratios showed a significant variation between the Liaodong Bay (0.185) and Bohai Strait (0.225), indicating that Pu derived from the Pacific Proving Grounds might have been transported to the Bohai Strait but not yet to the Liaodong Bay, which could further provide valuable reference for evaluating the seawater exchange cycle between the Bohai Sea and Yellow Sea.

The vertical distribution of plutonium 241Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, 241Pu/239+240Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of 241Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of 241Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident.

Presented have been the results of inventory estimation of anthropogenic beta-emitting ²⁴¹Pu, in different components in the southern Baltic Sea ecosystem. The total ²⁴¹Pu activity present in the Gulf of Gdańsk and the Gdańsk Basin for 2021 was estimated at 1.99 TBq and 7.82 TBq, respectively, of which 1.59 TBq and 6.38 TBq in the sediments. The Vistula and the Neman River and the atmospheric fallout were distinguished as the primary sources of plutonium in these basins. In seawater of the Gulf of Gdańsk, there was about 0.40 TBq ²⁴¹Pu (20.1% of total activity) and 1.44 TBq ²⁴¹Pu (18.4% of total activity) in the Gdańsk Basin. The ²⁴¹Pu accumulated in living organisms in 2021 was 1.13 GBq in the Gulf of Gdańsk and 3.96 GBq in the Gdańsk Basin. In the Gulf of Gdańsk biota, 55.7% was accumulated in zoobenthos, while in the Gdańsk Basin, 48.3% was in zoobenthos.

This study reviews the current understanding of the inventory and sources of plutonium (Pu) in the marine environment adjacent to China. The ²³⁹⁺²⁴⁰Pu inventory in the China Seas was found to have large spatial variations. The quantity in sediments decreases away from the shore, generally tracing the sedimentation rate distribution. High ²³⁹⁺²⁴⁰Pu inventories indicated that Pu in the water column was easily scavenged since Pu has a high particle affinity. Indeed, substantially higher ²⁴⁰Pu/²³⁹Pu atom ratios were observed in the sediment and seawater of the China Seas than are found in global fallout. We thus clarified that Pu sources in the China Seas were from both global fallout and the Pacific Proving Grounds (PPG) in the Pacific Marshall Islands. Plutonium from the latter source is transported into the China Seas through the North Equatorial Current (NEC) and Kuroshio. Using a two end-member mixing model, we revealed that the contribution of Pu from the PPG accounts for over 40% of the Pu in the East China Sea (ECS) and South China Sea (SCS), and less than 20% of the Pu in the Yellow Sea (YS). The distributions and isotopic composition of Pu in the China Seas indicate strong scavenging of Pu in the ECS and high Pu accumulation in the SCS. This information on the inventory and isotopic composition of Pu helps to establish a background for the future study of Pu in the China Seas.